arXiv subjects

A. K. Tyagi

Publications and source records attributed to A. K. Tyagi.

At least 19 recordsLinked to original sources

arXiv2019

Electronic properties of A2Zr2O7 (A= Gd, Nd) ceramic

The density functional theory with generalized gradient approximation has been used to investigate the electronic structure of gadolinium pyrochlore A2Zr2O7 (A=Gd, Nd) ceramic synthesized in polycrystalline form by solid state reaction. Structural characterization of the compound was done through X-ray diffraction (XRD) followed by Rietveld analysis of the XRD pattern. The Zr-K edge X-ray absorption (XAFS) spectra of A2Zr2O7 (A=Gd, Nd) were analysed together with those Zr-foil, which was used as reference compounds. X-ray photoemission spectroscopy (XPS), X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) for A2Zr2O7 (A=Gd, Nd) has been employed to obtain quantitative structural information on the Zr-local environment. The band gap is estimated using UV-Vis spectroscopy. The crystal structure is face centered cubic, space group being Fd-3m (No. 227). The total energies in this work were calculated using the generalized gradient approximation to DFT plus on-site repulsion (U) method.

cond-mat.mtrl-sci↗

arXiv2018

Enhanced radiation tolerance of YSZ at high temperature against swift heavy ions: key role of interplay between material microstructure and irradiation temperature

Yttria stabilized Zirconia (YSZ) pellets with different crystallite sizes were irradiated with 80 MeV Ag$^{6+}$ ions at room temperature and 1000 K to understand the role of crystallite size/material microstructure and irradiation temperature on the radiation tolerance against high electronic energy loss (S$_e$). X-ray diffraction and Raman spectroscopy measurements reveal that, irrespective of the irradiation temperature, the nano-crystalline samples suffered more damage as compared to the bulk-like sample. A reduction in the irradiation damage i.e. improvement in the radiation tolerance, was observed for all the samples irradiated at 1000 K. The reduction in the damage, however, was remarkably higher for the two nano-crystalline samples compared to the bulk-like sample, and hence the difference in the damage between the bulk-like and nano-crystalline samples was also significantly lower at 1000 K than that at room temperature. The irradiation damage, against S$_e$, was thus found to be critically dependent on the interplay between the irradiation temperature and crystallite size. These results are explained with the help of detailed theoretical calculations/simulations based on the 'in-elastic thermal spike' model by taking into consideration the combined effect of crystallite size and environmental (irradiation) temperature on the electron-phonon coupling factor and lattice thermal conductivity (and hence on the resulting thermal spike). Our results are crucial from the fundamental perspective of comprehending the size and temperature dependent radiation damage against S$_e$ ; and also for a number of applications, in various radiation environments, where nano-materials are being envisioned for use.

cond-mat.mtrl-sci↗

arXiv2017

Flipping growth orientation of nanographitic structures by plasma enhanced chemical vapor deposition

Nanographitic structures (NGSs) with multitude of morphological features are grown on SiO2/Si substrates by electron cyclotron resonance - plasma enhanced chemical vapor deposition (ECR-PECVD). CH4 is used as source gas with Ar and H2 as dilutants. Field emission scanning electron microscopy, high resolution transmission electron microscopy (HRTEM) and Raman spectroscopy are used to study the structural and morphological features of the grown films. Herein, we demonstrate, how the morphology can be tuned from planar to vertical structure using single control parameter namely, dilution of CH4 with Ar and/or H2. Our results show that the competitive growth and etching processes dictate the morphology of the NGSs. While Ar-rich composition favors vertically oriented graphene nanosheets, H2-rich composition aids growth of planar films. Raman analysis reveals dilution of CH4 with either Ar or H2 or in combination helps to improve the structural quality of the films. Line shape analysis of Raman 2D band shows nearly symmetric Lorentzian profile which confirms the turbostratic nature of the grown NGSs. Further, this aspect is elucidated by HRTEM studies by observing elliptical diffraction pattern. Based on these experiments, a comprehensive understanding is obtained on the growth and structural properties of NGSs grown over a wide range of feedstock compositions.

cond-mat.mtrl-sci↗

arXiv2017

The role of substrate bias and nitrogen doping on the structural evolution and local elastic modulus of diamond-like carbon films

Diamond-like carbon (DLC) films are synthesized on Si using plasma enhanced chemical vapor deposition. The role of substrate bias and nitrogen doping on the structural evolution and local elastic modulus of DLC films are systematically investigated. Raman spectroscopic studies reveal that the amount of graphitic C=C sp2 bonding increases with substrate bias and nitrogen doping. The density and hydrogen concentration in the films are found to vary from 0.7 to 2.2 g/cm3 and 16 to 38 atomic %, respectively, depending upon the substrate bias and nitrogen concentration in the DLC films. Atomic force acoustic microscopic (AFAM) analysis shows a direct correlation between local elastic modulus and structural properties estimated by Raman spectroscopy, Rutherford back scattering and elastic recoil detection analysis. AFAM analysis further confirms the evolution of soft second phases at high substrate biases (> -150V) in undoped DLC films. Further, N doping leads to formation of such soft second phases in DLC films even at lower substrate bias of -100 V. The AFAM studies provide a direct microscopic evidence for the "sub-implantation growth model" which predicts the formation of graphitic second phases in DLC matrix at high substrate biases.

cond-mat.mtrl-sci↗

arXiv2016

Geometrically frustrated GdInO$_3$: An exotic system to study negative thermal expansion and spin-lattice coupling

In this article, we report negative thermal expansion and spin frustration in hexagonal GdInO$_{3}$. Rietveld refinement of the XRD patterns reveal that the negative thermal expansion in the temperature range of 50-100K stems from the triangular lattice of Gd$^{3+}$ ions. At low temperature, the downward deviation of the inverse susceptibility ($χ^{-1}$) vs. $T$ plot from the Curie-Weiss law indicates spin frustration which inhibits long-range magnetic ordering down to 2K. Magnetostriction measurements clearly demonstrate a strong spin-lattice coupling. Low temperature anomalous phonon softening, as obtained from temperature dependent Raman measurements, also reveals the same. Our experimental observations are supported by first principles density functional theory calculations of the electronic and phonon dispersion of GdInO$_3$. The calculations suggest that the GdInO$_3$ lattice is highly frustrated at low temperature. Further, the calculated normal mode frequencies of the Gd related $Γ$ point phonons are found to depend on the magnetic structure of the lattice, suggesting significant magneto-elastic coupling.

cond-mat.mtrl-sci↗

arXiv2016

A comparative study on defect estimation using XPS and Raman spectroscopy in few layer nanographitic structures

Defects in planar and vertically oriented nanographitic structures (NGSs) synthesized by plasma enhanced chemical vapor deposition (PECVD) has been investigated using Raman and X-ray photoelectron spectroscopy. While Raman spectra reveal the dominance of vacancy and boundary type defects respectively in vertical and planar NGSs, XPS provides additional information on vacancy related defect peaks at C 1s spectrum that originate from non-conjugated carbon atoms in hexagonal lattice. Although an excellent correlation prevails between these two techniques, our results show that estimation of surface defects by XPS is more accurate than Raman analysis. Nuances of these techniques are discussed in the context of assessing defects in nanographitic structures.

cond-mat.mtrl-sci↗

arXiv2016

Electrochemical supercapacitor performance of SnO2 quantum dots

Metal oxide nanostructures are widely used in energy applications like super capacitors and Li-on battery. Smaller size nanocrystals show better stability, low ion diffusion time, higher-ion flux and low pulverization than bigger size nanocrystals during electrochemical operation. Studying the distinct properties of smaller size nanocrystals such as quantum dots (QDs) can improve the understanding on reasons behind the better performance and it will also help in using QDs or smaller size nanoparticles (NPs) more efficiently in different applications. Aqua stable pure SnO2 QDs with compositional stability and high surface to volume ratio are studied as an electrochemical super capacitor material and compared with bigger size NPs of size 25 nm. Electron energy-loss spectroscopic study of the QDs revealed dominant role of surface over the bulk. Temperature dependent study of low frequency Raman mode and defect Raman mode of QDs indicated no apparent volume change in the SnO2 QDs within the temperature range of 80-300 K. The specific capacitance of these high surface area and stable SnO2 QDs has showed only 9% loss while increasing the scan rate from 20 mV/S to 500 mV/S. Capacitance loss for the QDs is less than 2% after 1000 cycles of charging discharging, whereas for the 25 nm SnO2 NPs, the capacitance loss is 8% after 1000 cycles. Availability of excess open volume in QDs leading to no change in volume during the electro-chemical operation and good aqua stability is attributed to the better performance of QDs over bigger sized NPs.

cond-mat.mtrl-sci↗

arXiv2016

Localized Charge Transfer Process and Surface Band Bending in Methane Sensing by GaN Nanowires

The physicochemical processes at the surfaces of semiconductor nanostructures involved in electrochemical and sensing devices are strongly influenced by the presence of intrinsic or extrinsic defects. To reveal the surface controlled sensing mechanism, intentional lattice oxygen defects are created on the surfaces of GaN nanowires for the elucidation of charge transfer process in methane (CH4) sensing. Experimental and simulation results of electron energy loss spectroscopy (EELS) studies on oxygen rich GaN nanowires confirmed the possible presence of 2(ON) and VGa-3ON defect complexes. A global resistive response for sensor devices of ensemble nanowires and a localized charge transfer process in single GaN nanowires are studied in situ scanning by Kelvin probe microscopy (SKPM). A localized charge transfer process, involving the VGa-3ON defect complex on nanowire surface is attributed in controlling the global gas sensing behavior of the oxygen rich ensemble GaN nanowires.

cond-mat.mtrl-sci↗

arXiv2016

Carrier mediated reduction of stiffness in nanoindented crystalline Si(100)

We report the observation of carrier mediated decrease in the stiffness of crystalline (c)-Si(100) under nanoindentation. The apparent elastic modulii of heavily dopes (1E21 cm-3) p- and n-type c-Si are observed to be lower by 5.-7.5 percent that the estimated value for intrinsic (1E14 cm-3) c-Si. The deviation observed with respect to elastic modulus remarkably matches with the estimated value while considering the electronic elastic strain effect on carrier concentration as an influence of negative pressure coefficient of band gap for Si. The value is predominantly higher than the reported value of a decrease of 1-3 percent in stiffness as an effect of impurity in c-Si.

cond-mat.mtrl-sci↗

arXiv2016

Localized tip enhanced Raman spectroscopic study of impurity incorporated single GaN nanowire in the sub-diffraction limit

The localized effect of impurities in single GaN nanowires in the sub-diffraction limit is reported using the study of lattice vibrational modes in the evanescent field of Au nanoparticle assisted tip enhanced Raman spectroscopy (TERS). GaN nanowires with the O impurity and the Mg dopants were grown by the chemical vapor deposition technique in the catalyst assisted vapor-liquid-solid process. Symmetry allowed Raman modes of wurtzite GaN are observed for undoped and doped nanowires. Unusually very strong intensity of the non-zone center zone boundary mode is observed for the TERS studies of both the undoped and the Mg doped GaN single nanowires. Surface optical mode of A1 symmetry is also observed for both the undoped and the Mg doped GaN samples. A strong coupling of longitudinal optical (LO) phonons with free electrons, however is reported only in the O rich single nanowires with the asymmetric A1(LO) mode. Study of the local vibration mode shows the presence of Mg as dopant in the single GaN nanowires.

cond-mat.mtrl-sci↗

arXiv2016

Nonpolar p-GaN/n-Si heterojunction diode characteristics: A comparison between ensemble and single nanowire devices

The electrical and photodiode characteristics of ensemble and single p-GaN nanowire and n-Si heterojunction devices were studied. Ideality factor of the single nanowire p-GaN/n-Si device was found to be about three times lower compared to that of the ensemble nanowire device. Apart from the deep-level traps in p-GaN nanowires, defect states due to inhomogeneity in Mg dopants in the ensemble nanowire device are attributed to the origin of high ideality factor. Photovoltaic mode of ensemble nanowire device showed an improvement in the fill-factors up to 60 percent over the single nanowire device with fill-factors up to 30 percent. Reponsivity of the single nanowire device in photoconducting mode was found to be enhanced by five orders, at 470 nm. The enhanced photoresponse of the single nanowire device also confirms the photoconduction due to defect states in p-GaN nanowires.

cond-mat.mtrl-sci↗

arXiv2016

Optical band gap and associated band-tails in nanocrystalline AlN thin films grown by reactive IBSD at different substrate temperatures

AlN thin films have been grown on Si (100) substrates by reactive ion beam sputter deposition (IBSD) at different substrate temperatures varying from room temperature (RT) to 500oC. Substrate temperature induced microstructural transition from amorphous at RT, nanocrystalline at 300oC to microcrystalline at 400oC has been observed by Transmission Electron Microscopy (TEM). Average surface roughness (Ra) and morphology has been explored by using Atomic Force Microscopy (AFM). UV-VIS spectrophotometry has been employed to probe the substrate temperature induced changes in optical band-gap (Eg) of grown thin films in reflectance mode. It was found that Eg was increased from 5.08 to 5.21 eV as substrate temperature was increased from RT to 500oC. Urbach energy tail (Eu) along with weak absorption tail (WAT) energy (Et) have been estimated to account for the optical disorder which was found to decrease with associated increase in Eg.

cond-mat.mtrl-sci↗

arXiv2015

XPS studies on AlN thin films grown by ion beam sputtering in reactive assistance of N+/N2+ ions: Substrate temperature induced compositional variations

We report on an XPS study of AlN thin films grown on Si(100) substrates by ion beam sputter deposition (IBSD) in reactive assistance of N+/N2+ ions to unravel the compositional variation of their surface when deposited at different substrate temperatures. The temperature of the substrate was varied as room temperature (RT), 100oC and 500oC. The binding energy of Al-2p, N-1s and O-1s core electrons indicate the formation of 2H polytypoid of AlN. The increase in concentration of AlN with substrate temperature during deposition is elucidated through detailed analysis with calculated elemental atomic concentrations (at. %) of all possible phases at the film surface. Our results show that predominate formation of AlN as high as 74 at. % is achievable using substrate temperature as the only process parameter. This high fraction of AlN in thin film surface composition is remarkable when compared to other growth techniques. Also, the formation of other phases is established based on their elemental concentrations.

cond-mat.mtrl-sci↗

arXiv2015

Novel single phase vanadium dioxide nanostructured films for methane sensing near room temperature

Methane (CH_4) gas sensing properties of novel vanadium dioxide (VO_2) nanostructured films is reported for the first time. The single phase nanostructures are synthesized by pulsed dc-magnetron sputtering of V target followed by oxidation in O_2 atmosphere at 550 ^oC. The partial pressure of O_2 is controlled to obtain stoichiometric VO_2 with the samples showing rutile monoclinic crystalline symmetry and regions of rod shaped nano-architectures. These nanostructured films exhibit a reversible semiconductor to metal transition in the temperature range of 60-70 ^oC. Gas sensing experiments are carried out in the temperature span from 25 ^oC to 200 ^oC in presence of CH_4. These experiments reveal that the films respond very well at temperatures as low as 50 ^oC, in the semiconducting state.

cond-mat.mtrl-sci↗

arXiv2015

Optical Properties of Mono-Dispersed AlGaN Nanowires in the Single-Prong Growth Mechanism

Growth of mono-dispersed AlGaN nanowires of ternary wurtzite phase is reported using chemical vapour deposition technique in the vapour-liquid-solid process. The role of distribution of Au catalyst nanoparticles on the size and the shape of AlGaN nanowires are discussed. These variations in the morphology of the nanowires are understood invoking Ostwald ripening of Au catalyst nanoparticles at high temperature followed by the effect of single and multi-prong growth mechanism. Energy-filtered transmission electron microscopy is used as an evidence for the presence of Al in the as-prepared samples. A significant blue shift of the band gap, in the absence of quantum confinement effect in the nanowires with diameter about 100 nm, is used as a supportive evidence for the AlGaN alloy formation. Polarized resonance Raman spectroscopy with strong electron-phonon coupling along with optical confinement due to the dielectric contrast of nanowire with respect to that of surrounding media are adopted to understand the crystalline orientation of a single nanowire in the sub-diffraction limit of about 100 nm using 325 nm wavelength, for the first time. The results are compared with the structural analysis using high resolution transmission microscopic study.

cond-mat.mtrl-sci↗

arXiv2015

Invoking forbidden modes in SnO_2 nanoparticles using tip enhanced Raman spectroscopy

Raman forbidden modes and surface defect related Raman features in SnO_2 nanostructures carry information about disorder and surface defects which strongly influence important technological applications like catalysis and sensing. Due to the weak intensities of these peaks, it is difficult to identify these features by using conventional Raman spectroscopy. Tip enhanced Raman spectroscopy (TERS) studies conducted on SnO_2 nanoparticles (NPs) of size 4 and 25 nm have offered significant insights of prevalent defects and disorders. Along with one order enhancement in symmetry allowed Raman modes, new peaks related to disorder and surface defects of SnO_2 NPs were found with significant intensity. Temperature dependent Raman studies were also carried out for these NPs and correlated with the TERS spectra. For quasi-quantum dot sized 4 nm NPs, the TERS study was found to be the best technique to probe the finite size related Raman forbidden modes.

cond-mat.mtrl-sci↗

arXiv2015

Raoult's Formalism in Understanding Low Temperature Growth of GaN Nanowires using Binary Precursor

Growth of GaN nanowires are carried out via metal initiated vapor-liquid-solid mechanism, with Au as the catalyst. In chemical vapour deposition technique, GaN nanowires are usually grown at high temperatures in the range of 900-1100 ^oC because of low vapor pressure of Ga below 900 ^oC. In the present study, we have grown the GaN nanowires at a temperature, as low as 700 ^oC. Role of indium in the reduction of growth temperature is discussed in the ambit of Raoult's law. Indium is used to increase the vapor pressure of the Ga sufficiently to evaporate even at low temperature initiating the growth of GaN nanowires. In addition to the studies related to structural and vibrational properties, optical properties of the grown nanowires are also reported for detailed structural analysis.

cond-mat.mtrl-sci↗

arXiv2015

Growth of InN quantum dots to nanorods: A competition between nucleation and growth rates

Growth evolution of InN nanostructures via a chemical vapor deposition technique is reported using In_2O_3 as precursor material and NH_3 as reactive gas in the temperature range of 550-700 ^oC. Morphology of the nanostructures solely depends on the growth temperature, evolving from quantum dot sized nanoparticles to nanorods. It is found that 630 ^oC is the threshold temperature for nanorod growth. At 630 ^oC, nucleation starts with multifaceted particle having {10-12} surface planes. Subsequently, hexagonal polyhedral NRs are grown along the [0001] direction with non-polar surfaces of m-planes {10-10}. A comprehensive study is carried out to understand the evolution of nanorods as a function of growth parameters like temperature, time and gas flow rate. Change in the morphology of nanostructures is explained based on the nucleation rate and the growth rates during the phase formation. Raman studies of these nanostructures show that a biaxial strain is developed because of unintentional impurity doping with the increase in growth temperature.

cond-mat.mtrl-sci↗